In recent years, we have explored non-amide-based classes of kinetic hydrate inhibitor (KHI) polymers to determine if the same level of performance can be achieved as commercial KHI polymers, which all contain amide groups. Here, we have investigated a series of polyvinylaminals as KHIs for the first time. These polymers with pendant alkyl or cycloalkyl groups of varying sizes and shapes were synthesized in a simple one-step procedure from polyvinylamine. Their performance as tetrahydrofuran (THF) hydrate crystal growth inhibitors and as high-pressure KHIs was studied with a structure II-forming natural gas mixture in both sapphire and steel rocking cells. A structure-performance analysis was carried out. The best KHI was obtained with a polyvinylaminal with pendant cyclohexyl groups and gave a similar performance to the well-known KHI poly(N-vinyl caprolactam) and without the disadvantage of a low cloud point.