Can you relate an existing Account or Contact to an Opportunity using a Workflow?

We are looking to use a Workflow to relate an existing Account (based on email domain) or Contact (based on email) to an Opportunity on save. Is this possible? I have been looking but not found anyone asking the question - sorry if I have missed something!
Thank you for your help,

If you use logic hooks, before_save, it is possible.
Via Workflow, i don’t know. if you can share more details/screenshots, what fields you have in opportunity, how have you setup any existing workflow that you tried.

Relationships are possible by workflow. Here’s an example of where I create a planned call for a new lead and relate it to the lead by ContactID. You can relate the source module to pretty much any other module as long as an established relationship exists. In this case I’m creating a call record with the workflow and relating it to the lead, but you can also Modify a Record and add the relationship.

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