For mail, a few things I'd look for:
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Standard protocol compatibility (POP/IMAP/JMAP/SMTP) so you can use a client that's not controlled by the service provider.
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Easy E2EE setup with PGP/GPG.
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Custom domain support.
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Email alias support (though this can be done with a third-party service, potentially).
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Server-side filter rules for incoming mail.
Proton and Tuta, for example, fail on point #1. The E2EE promise really doesn't mean a lot when the service provider ultimately controls the client. If they control the client, they could very easily exfiltrate your keys via a backdoor. This can be mitigated with open-source clients and reproducible builds, but if you're using a web client or apps from Google/Apple stores, that's never going to be verifiable.
For VPN:
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No-logs policy.
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Independent audits.
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Port forwarding support.
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Anonymous payment options.
These are not exhaustive lists, just off the top of my head.
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