Spodoptera frugiperda J. E. Smith (Lepidoptera: Noctuidae) (fall armyworm) is a pest native to the Americas that affects a variety of crops. Its control is based on chemical insecticides. However, this practice has been associated with changes in the susceptibility of pests to various insecticides. The use of plant products represents an eco-friendly alternative. The objective of this work was to evaluate the larvicidal activity of the chloroform extract of Senna crotalarioides (Kunth) H.S. Irwin & Barneby (Fabaceae) to control S. frugiperda. The chloroform extract of S. crotalarioides caused significant larval mortality, and reduced pupal weight and adult emergence. The analysis by gas chromatography coupled with mass spectrometry (GC-MS) revealed the presence of 22 compounds in the chloroform extract of S. crotalarioides leaves, with the straight-chain aliphatic fatty alcohol 1-octacosanol as the main component. This study revealed that the leaves of S. crotalarioides synthesize long chain alcohols, which increased the mortality of S. frugiperda in its larval stage, including the pupal stage. The extract also caused a decrease in the S. frugiperda pupal weight. The potential use of the chloroform extract obtained from S. crotalarioides and its principal chemical constituent is proposed as a promising alternative to control S. frugiperda.