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You should be able to add a key binding with the User Interface > Keyboard > Custom Key Bindings preference and set the command to:

set-current-as-main-entry-point

However, this does not clear the main entry point if the current file is already the main entry point. That could be done with another key binding for the command clear-project-main-entry-point

If you wanted to create a binding that exactly matches what you wrote, the only way would be to write an extension script to implement that functionality and then bind it to a key.