How to see only photos NOT in an album

Which system version do you have installed? The option "Any" has only been available in macOS 10.14 Mojave or later. On macOS 10.15 and macOS 11 the smart album did not work properly, but it seems to be fixed in BigSur or later: Problems with the Smart Album Rule: Album is not Any in Photos 5.0 - Apple Community

If you are using iCloud Photos you can clean up your Library by moving the photos you have organized in albums to the Shared iCloud Photos Library (if you do not need the Shared Library for Sharing with family and friends). See: Using the Shared iCloud Photos Library to have two separate libraries on all devices - Apple Community

Since macOS 13 Ventura our iCloud Photos Library can be split into a personal library and a shared library, and we can switch easily with a click on the selector between the two libraries, or view both together. The shared library will be available on all devices signed into your AppleID.

To organize your albums you could do the following:

• Set up a shared iCloud Photos Library, if you have not yet done so. How to use iCloud Shared Photo Library - Apple Support
• Set the selector in the toolbar to view your Personal Library.
• Select all photos in an album and move them to the Shared Library. To move selected photos to the Shared iCloud Library ctrl-click them and use the command "Move to Shared Library". You will still be seeing the photos in their respective albums, when you are setting the selector to "Shared Library" or both Libraries", but are no ,longer visible in the Personal Library.

When all albums in your personal library appear to be empty, you will only be seeing the photos not in any albums in your Personal library. You are now having two separate sections of your Photos Library in iCloud - the well organised show-case "Shared iCloud Photos Library" and the construction site "Personal Library".

Essentially, the toggle switch to switch between the Shared iCloud Photos Library and the personal Library is a custom filter. On a Mac, we could do the same with keywords, but the advantage of the Shared Library is, that we can use it directly at icloud.com and all our mobile denied (iPhone, iPad, Apple Vision One) as well.

You can use this method, if all your devices are compatible with the Shared iCloud Photos Library, and if you are not using your Shared Library for Sharing with others. I would not use it for this purpose anyway. My iCloud Photos Library is my most important library and would not leave someone to the mercy of others who could flood it with each and every photo they take right from the camera, or delete or modify my photos or their metadata. It would be a nightmare. Things to consider when setting up the Shared iCloud Photos Library in Photo 8 on Ventura

The available choices in the middle and right columns are determined by the selections to the left. Make sure you select "Album" on the right and "is not" in the middle before you try to select "Any" on the right.

If it still doesn't work for you, let us know what version of Photos you are using.

It's not a feature available on iOS.

Photos, (like iPhoto, Aperture, Music, iTunes) is a database. This means it can be very flexible and powerful, if sometimes a little confusing. The library is the core of the app. Every image is in the library. Albums are virtual, and are just subsets of the library. In fact, Albums are not places, they are lists - instructions to the app to 'display this group of images together'. So images do not get "moved" to Albums, they get added to that particular list. This means that an image can be in more than one album but use no extra disk space. Similarly in the Music app, all the tracks are in the Library and can be added to any number of playlists.

Photos for Mac has a smart album feature that will find all the image sin your Library that are not in album, but that's not on iOS. Feature requests go here:

Feedback - Photos - Apple

Have you tried this:

The right hand drop-down on my Mac doesn't have the "Any" option.

Yer_Man didn't answer the question.

"Photos for Mac has a smart album feature that will find all the image sin your Library that are not in album"

Really? I don't see it. When I select "new smart album" in Photos, I do not see any "feature" that will find all images not in an album.

Can anyone provide more details?

Thx!