Natural products have long been used as pharmaceutical actives for the treatment of diseases. More recently, natural products with the ability to self‐assemble to form soft material‐gels, i.e. natural product gelators (NPGs), were discovered. This subverts our traditional insight into natural products as drugs and drives us to elucidate how NPGs form gels. Here, we interpret “why gel” from the perspective of solvents based on the basic theory of thermodynamics for liquids, and then propose the hypothesis of solvent‐induced gel formation in combination with the NPGs with polycyclic structures. This hypothesis provides a complete explanation of how the gelator and solvent play a role in the overall gel formation and helps us to more easily understand the gelation.