Yes, you can go to Settings, select Security, and when you toggle off Allow auto-assign as a site collection administrator when required you will get a prompt with a button to remove the permissions.
If you have Only on selected connections selected, disabling an environment or service where you were previously added as a site collection admin will give you the option to remove the admin permissions for that specific environment or service.
If you require more granular control over the remove operation, you can remove your account as a site collection admin with a custom report with the steps below:
- Select All reports from the menu.
- Click Create custom report.
- Select OneDrive for Business or Site collection as your Object type (depending on your scenario).
- Click Continue without saving.
- Specify your target(s).
- Click Next.
- Click Run now.
- Select all results using the top-left checkbox.
- Click Remove permissions in the Quick actions menu.
- In the Select users or groups field, input yourself or any other applicable user who you are removing administrative rights from.
- Use the Remove permissions drop-down to select Remove from site collection administrators.
- Click Apply.
- You will now see the results page.
Note: If you are using a custom report, make sure you disable the auto-assign feature first. The app will add your account whenever you run operations on your sites or when it crawls your environment if you don't disable the feature.