diff --git a/src/material/core/option/option.ts b/src/material/core/option/option.ts
index 2f427ff9b256..bc159afce814 100644
--- a/src/material/core/option/option.ts
+++ b/src/material/core/option/option.ts
@@ -204,16 +204,6 @@ export class _MatOptionBase<T = any> implements FocusableOption, AfterViewChecke
     }
   }
 
-  /**
-   * Gets the `aria-selected` value for the option. We explicitly omit the `aria-selected`
-   * attribute from single-selection, unselected options. Including the `aria-selected="false"`
-   * attributes adds a significant amount of noise to screen-reader users without providing useful
-   * information.
-   */
-  _getAriaSelected(): boolean | null {
-    return this.selected || (this.multiple ? false : null);
-  }
-
   /** Returns the correct tabindex for the option depending on disabled state. */
   _getTabIndex(): string {
     return this.disabled ? '-1' : '0';
@@ -267,7 +257,16 @@ export class _MatOptionBase<T = any> implements FocusableOption, AfterViewChecke
     '[class.mat-mdc-option-active]': 'active',
     '[class.mdc-list-item--disabled]': 'disabled',
     '[id]': 'id',
-    '[attr.aria-selected]': '_getAriaSelected()',
+    // Set aria-selected to false for non-selected items and true for selected items. Conform to
+    // [WAI ARIA Listbox authoring practices guide](
+    //  https://www.w3.org/WAI/ARIA/apg/patterns/listbox/), "If any options are selected, each
+    // selected option has either aria-selected or aria-checked  set to true. All options that are
+    // selectable but not selected have either aria-selected or aria-checked set to false." Align
+    // aria-selected implementation of Chips and List components.
+    //
+    // Set `aria-selected="false"` on not-selected listbox options to fix VoiceOver announcing
+    // every option as "selected" (#21491).
+    '[attr.aria-selected]': 'selected',
     '[attr.aria-disabled]': 'disabled.toString()',
     '(click)': '_selectViaInteraction()',
     '(keydown)': '_handleKeydown($event)',
diff --git a/src/material/legacy-core/option/option.ts b/src/material/legacy-core/option/option.ts
index 696af7fcf96f..c2ab6d03f9f9 100644
--- a/src/material/legacy-core/option/option.ts
+++ b/src/material/legacy-core/option/option.ts
@@ -38,7 +38,7 @@ import {MatLegacyOptgroup} from './optgroup';
     '[class.mat-option-multiple]': 'multiple',
     '[class.mat-active]': 'active',
     '[id]': 'id',
-    '[attr.aria-selected]': '_getAriaSelected()',
+    '[attr.aria-selected]': 'selected',
     '[attr.aria-disabled]': 'disabled.toString()',
     '[class.mat-option-disabled]': 'disabled',
     '(click)': '_selectViaInteraction()',
diff --git a/src/material/legacy-select/select.spec.ts b/src/material/legacy-select/select.spec.ts
index 829e409d1425..68d9625ea80b 100644
--- a/src/material/legacy-select/select.spec.ts
+++ b/src/material/legacy-select/select.spec.ts
@@ -1151,9 +1151,9 @@ describe('MatSelect', () => {
         }));
 
         it('should set aria-selected on each option for single select', fakeAsync(() => {
-          expect(options.every(option => !option.hasAttribute('aria-selected')))
+          expect(options.every(option => option.getAttribute('aria-selected') === 'false'))
             .withContext(
-              'Expected all unselected single-select options not to have ' + 'aria-selected set.',
+              'Expected all unselected single-select options to have aria-selected="false".',
             )
             .toBe(true);
 
@@ -1168,9 +1168,9 @@ describe('MatSelect', () => {
             .withContext('Expected selected single-select option to have aria-selected="true".')
             .toEqual('true');
           options.splice(1, 1);
-          expect(options.every(option => !option.hasAttribute('aria-selected')))
+          expect(options.every(option => option.getAttribute('aria-selected') === 'false'))
             .withContext(
-              'Expected all unselected single-select options not to have ' + 'aria-selected set.',
+              'Expected all unselected single-select options to have aria-selected="false".',
             )
             .toBe(true);
         }));
diff --git a/src/material/select/select.spec.ts b/src/material/select/select.spec.ts
index 3a541e180ffa..7990116a5542 100644
--- a/src/material/select/select.spec.ts
+++ b/src/material/select/select.spec.ts
@@ -1184,9 +1184,9 @@ describe('MDC-based MatSelect', () => {
         }));
 
         it('should set aria-selected on each option for single select', fakeAsync(() => {
-          expect(options.every(option => !option.hasAttribute('aria-selected')))
+          expect(options.every(option => option.getAttribute('aria-selected') === 'false'))
             .withContext(
-              'Expected all unselected single-select options not to have ' + 'aria-selected set.',
+              'Expected all unselected single-select options to have ' + 'aria-selected="false".',
             )
             .toBe(true);
 
@@ -1203,9 +1203,9 @@ describe('MDC-based MatSelect', () => {
             )
             .toEqual('true');
           options.splice(1, 1);
-          expect(options.every(option => !option.hasAttribute('aria-selected')))
+          expect(options.every(option => option.getAttribute('aria-selected') === 'false'))
             .withContext(
-              'Expected all unselected single-select options not to have ' + 'aria-selected set.',
+              'Expected all unselected single-select options to have ' + 'aria-selected="false".',
             )
             .toBe(true);
         }));
diff --git a/tools/public_api_guard/material/core.md b/tools/public_api_guard/material/core.md
index d636b62761f5..7c61bb0f327c 100644
--- a/tools/public_api_guard/material/core.md
+++ b/tools/public_api_guard/material/core.md
@@ -279,7 +279,6 @@ export class _MatOptionBase<T = any> implements FocusableOption, AfterViewChecke
     set disabled(value: BooleanInput);
     get disableRipple(): boolean;
     focus(_origin?: FocusOrigin, options?: FocusOptions): void;
-    _getAriaSelected(): boolean | null;
     _getHostElement(): HTMLElement;
     getLabel(): string;
     _getTabIndex(): string;