After they have been requested not to call anymore, any further calls are a violation of the TCPA. Companies that do not respect someone's right and notification to receive no more phone calls need to be sued into compliance. That is why the TCPA was established, to allow end users to claim damages against companies that refuse to stop calling. Continued calls after a notification to discontinue calling are grounds for a suit for $500 in damages for each additional phone call. Many companies try to skirt this by claiming they need 30, 60, even 90 days, to process a number removal request, and that they can continue calling. The TCPA gives them no provision for such delay. Many people have successfully sued telemarketers under the provisions of this law.
The "Do Not Call" registry, established by the newer "Telemarketing Sales Rule" (TSR), by comparison is merely a way for the government to levy a fee on telemarketers. As long as they pay the fees to "scrub" their list, any mistakes they make on continuing to call individuals who don't want to be called are covered by safe harbour provisions. The individuals receiving the calls get no right of recovery under the TSR, unless they can prove damages over $50,000. The TSR also makes requirements that the companies advertise proper caller ID on their calls, but they are regularly failing to do this, especially on illegal calls to cell phones, and the FCC and local phone companies do not care to do any enforcements other than compile statistics on how many people complain about the practice.
The TCPA is a simpler, older law, that puts reasonable sanctions in the hands of the individual. The "Do Not Call" registry is not nearly as end user focused.