無理する is often used to mean "do something unreasonable/work yourself excessively" (push yourself to wash in freezing cold water, for example). I think you've got the broad gist of the meaning.
Another example of a similar use of せずに would be something like this (遠慮する means to hold back, often out of politeness)
遠慮せずに食べてください
(lit. "without restraining yourself, please eat", more loosely like "feel free to dig in")