While you are on an active call in smrtPhone from the Chrome Extension, you have the option to flip directly to Podio and either view the call or view the lead.
When you click the 3 dots next to the Contact Name or Phone Number (⋮) you will get a menu of options including:
Mark as Spam - will add the number to your Spam List
View Call in Podio - will take you to your Communications App
Create Contact - an option that appears if the number is not in your Contacts App
View Lead in Podio - an option that appears if the contact is in your Contacts App
Update Existing Contact - allows you to add the number to an existing contact
This is what the menu looks like when the number you are on a call with is not in your Contacts App: