As far as I'm aware you can only sync on CRM at a time to one instance. You may be able to get some middleware that can sync the two into one but I don't believe Marketo does this as part of their package? Unless, of course, there has been a recent upgrade?
Basically there is a 1:1 relationship with Marketo and SFDC. 1 instance syncs to 1 instance.
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As others have confirmed, natively you can only have 1 CRM integration. However, many customers have 2+ lead partitions and use either a middleware tool (e.g. Boomi, Informatica, Mulesoft) or create a custom web service to sync this other lead partition to their other CRM.
This solution works well as long as you don't have the same record in both CRM's because then you would be using Marketo as a mediator pushing updates from one system to another which isn't ideal.
If it makes sense from a business perspective to use one instance of Marketo, you can hook it up to either SFDC or Dynamics CRM (just one) and I would suggest SFDC. And then you can use an integration tool to sync data between the synced CRM system and the other one.
We just finished a project here where 2 SFDC instances are used, 1 synced to Marketo and both synced to each other using Informatica Cloud and Informatica Cloud Real Time.
I've also had to deal with the multiple CRM instance challenge. Marketo's native connectors don't support this, but Bedrock Data is a third party tool for marketers to connect Marketo to multiple CRM instances, and manage the rules for which data syncs.