Dedicated to Prof. Gaetano Guerra on the occasion of his 60th birthday.The mechanisms responsible for the physical gelation of polymers and of organogelators are discussed and compared. For polymers, the prerequisite for obtaining fi brillar thermoreversible gels is the impediment of chain folding. This occurs when polymers take on a worm-like chain conformation with a large persistence length. This property can be intrinsic to the polymer, such as agarose, or can be obtained by the occurrence of polymer-solvent molecular compounds, as is the case for stereoregular polymers. For organogels, it is suggested that the mechanism for producing fi brils involves the much faster growth of one face of the organogel crystal structure with respect to the other two, which can be enhanced via specifi c interactions with the solvent, something reminiscent of molecular compounds.