Yes, Roger Penrose, despite his extraordinary career and contributions to science, has more recently been engaging more in this type of pseudoscience.
It can and has happened to other extraordinary minds as well - Linus Pauling, one of the forefathers of quantum chemistry and molecular biology, but also a promoter of vitamin C as a panacea in his later years.
GP asked whether we are calling what Roger Penrose is doing pseudoscience, and I responded that we do.
Now, why is it pseudoscience?
Because the parts of the theory due to Penrose are essentially philosophical, he doesn't really make any firm claims beyond "quantum effects - particularly superposition - are involved in human decision-making". The parts that Hameroff brings to the table are specific, but fanciful. The whole "microtubules observe quantum effects" is about as plausible as cold fusion - it is motivated thinking that contradicts some basic limits that we have observed, and relies on some gaps in our physical knowledge to not quite be provably wrong.
Overall they are combining musings about the universe with bits of biology and QM that are not yet fully understood into a theory that uses the trappings of science, but relies on motivated thinking to have any plausibility. It's most similar to the homeopathic quacks' claims about the memory of water: not fully proven to be impossible, but moatly on account of the vagueness of the claims. So, what they are doing fits the definition of pseudoscience.
Penrose and Hameroff's theory about microtubules is certainly science not pseudoscience. It is a specific theory with falsifiable predictions.
In the absence of a definition of consciousness, perhaps the only validation would be evidence that general anaesthetics take effect in the microtubules (Hameroff is an anaesthesiologist).
It might not be possible to show that macroscopic quantum effects are required, or that consciousness is more powerful than an algorithmic computer (Turing Machine) - two of Penrose's related speculations.
Another of Penrose's claims is that gravitational divergences collapse the quantum wavefunction. This is logically separate from, but is often linked with, the conscious perception issue, as presented in their Orchestrated Objective Reduction theory (ORR):
The latter gravitational claim is being tested independently from brains, using conventional QM experiments in the presence of large masses. The precision to resolve the question is within reach.
I have watched and read his opinions and yes, he has, in my opinion, veered into pseudoscience. It's not exactly without precedence for an established and respected scientist to go all philosophical with age.
I would put his current position somewhere like "I really want free will to be true therefore..." rather than an observational approach.
Penrose, like it or not, has developed a fairly rigorous, if not flawed hypothesis that is quite a stark contrast between many philosophers who espouse such ideas as pan psychism.
It can and has happened to other extraordinary minds as well - Linus Pauling, one of the forefathers of quantum chemistry and molecular biology, but also a promoter of vitamin C as a panacea in his later years.