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No, VCR can only record SD.

Although I believe you can use a digital converter/tuner.

What defines the definition in VCR tape? The size of the magnetic grains in the tape or something like that? Is it possible to manufacture a special magnetic VCR tape that could write DVD-quality definition?

In practice it'd just be the standard of the signal that's being recorded (PAL/NTSC/SECAM). Wouldn't surprise me if the actual tape is capable of handling more..

Consumer VHS VCRs could not reproduce the full fidelity of a broadcast NTSC picture. Commercial VCRs, which typically used Betamax, were better and used by broadcasters until digital took over.

The grains on the tape ultimately determine how high of a frequency it can record. And how close together the tracks can be.

yes and no. there is dvhs. But even though the medium looks like a standard vhs cassette it is a different technology.

https://en.wikipedia.org/wiki/D-VHS

Here is a video recorded on a dvhs in 1993. It aged rather well I think: https://www.youtube.com/watch?v=fT4lDU-QLUY

You would need to convert it to NTSC. Probably most set-top boxes still have a cable coax output on channel 3 or 4, which you could connect to your VCR.