The occurrence of gelation in certain crystallization systems is well known, but has rarely been used for fabricating drug-containing hydrogels with suitable properties such as controlled release. In this study, a novel gelation method using a drug was developed for the preparation of hydrogels with high drug contents of 60.90 wt% with easy drug loading onto the hydrogels. The antisolvent crystallization of atorvastatin (ATV) in the presence of polyacrylic acid (PAA) resulted in gelation without phase separation issues. On increasing the ATV/PAA ratio, the elastic modulus increased and the gelation time decreased, suggesting that the ATV crystallites act as physical crosslinks. The crystallinity and particle size of ATV and the release kinetics could be controlled over a wide window. This simple gelation technique could be useful in the future development of controlled release formulations via cost-efficient processes.