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I have applied to multiple firms many of which have never responded (even after updates and emails expressing a continued interest). Is is appropriate to call or send a letter via the mail to follow up?

I just feel at some point the communication goes from showing initiative to being harassing. And absolutely do not want to fall into the harassment category.

Thanks in advance!

Law firms are major businesses. They will get back to you when - and if - they so desire. Your mail isn't lost and pestering them isn't going to help.

You can follow up if you want, but hearing nothing, or hearing nothing for long stretches of time, is standard operating procedure.