A number of soybean varieties traditionally bred for resistance to various soybean arthropod pests have been identified as resistant to Megacopta cribraria (F.) (Hemiptera: Plataspidae). However, the mechanisms of host-plant resistance (HPR) in this system are not understood. The goal of this study was to identify the mechanisms of resistance by examining the role of plant volatile organic compounds (VOCs) and free amino acids (FAAs) among 16 soybean varieties. Choice and no-choice cage experiments identified several soybean varieties that demonstrated antixenosis as well as antibiosis. However, resistance varied over time in certain soybean varieties, such as N02-7002 and PI567352B. Mean nymph number from choice experiments had positive correlations with the FAAs asparagine, tryptophan, alanine, phenylanaline, and serine; negative correlation with leucine and threonine. Four plant volatiles, hexanal, 2-pentylfuran, beta-cyclocitral, and cis-9-hexadecenal, were positively correlated with subsequent nymph development, whereas n-hexadecenoic acid was negatively correlated with nymph number only, in adult choice cage experiments. This study contributes to understanding the mechanisms of HPR through associations with plant VOCs and FAAs in relation to M. cribraria development and provides useful knowledge for developing soybean varieties for M. cribraria management.