I don't have any experience with version control from the terminal but as far as I can tell SmartGit does not have a terminal nor does it use an external git client that I could configure via terminal so I don't really see how I can execute git configuration commands on it. Specifically, I want to do:
git config --global core.autocrlf true
Does it have an equivalent configuration option available from within the UI or is there some other way to apply this?
SmartGit/Hg uses the command line Git which is configured in the Preferences. Both, command line Git and SmartGit/Hg will honor the global core.autocrlf configuration from your .gitconfig file.