The behavioral inhibition system (BIS) and behavioral activation system (BAS) are hypothesized to underlie motivated behavior, relate to hippocampal and amygdalar function, and link to pathological gambling (PG). Prior studies have not investigated hippocampal and amygdalar volumes in PG and their relationships to BIS/BAS measures. Structural MRI scans and BIS/BAS and other clinical measures were obtained from 32 PG individuals and 47 healthy comparison (HC) individuals. Volumetric measures of the hippocampus and amygdala were assessed using FreeSurfer and related to BIS/BAS measures. PG relative to HC individuals demonstrated diminished volume in the left hippocampus and right amygdala and higher BIS and BAS scores. BIS scores were positively correlated with left hippocampal and left amygdalar volumes in PG individuals. The findings of relatively diminished hippocampal and amygdalar volumes in PG individuals resonate with findings from substance-dependent groups. Relationships between amygdalar and hippocampal volumes and BIS measures in PG suggest that individual differences in these structures may contribute to avoidance behaviors in PG.