I have a TN visa (mexican citizen) that was renewed on Nov '13, thus will expire on Nov '14. But I accepted a job back on Mexico and already quit my US employeer. Now I'm living on Mexico. How can I cancel my current TN visa? and what should I do with the I-94?
You should have returned the I 94 to the airline upon your departure flight from the US. If it is through the port of entry that you left either on foot or by car, then make sure to save everything and proof of your having started to work and live in Mexico. You may want to return to the port of entry and surrender your I 94 to CBP, with proof of your having lived and worked in Mexico since, you do not want the CBP and USCIS databases to have a record of you having never left the US after the date of your TN's expiration.
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Now that you are back in Mexico, there is no need for you to do either.
Mr. Shusterman's (former INS Trial Attorney, 1976-82) response to your question is general in nature, as not all the facts are known to him. You should retain an attorney experienced in immigration law to review all the facts in your case in order to receive advice specific to your case. Mr. Shusterman's statement above does not create an attorney/client relationship.
Criminal Defense Attorney
If you already accepted the new employment and already terminated your employment in the US you do not have to cancel your prior TN visa and just let it expire by its expiration date if you so desire.
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You do not need to cancel or do anything. By leaving the employer that "cancel" the visa and status. Unless, of course you want to go back them and then the visa can be used again.