In cross-linguistic word learning, learning new knowledge based on existing knowledge is a common and lifelong process. This study investigated whether inhibitory control would be conducive to this process. We asked Chinese-English bilinguals to learn new meanings for familiar English ambiguous words within two consecutive days, manipulating semantic relatedness and word frequency to create four categories: high-frequency-unrelated, high-frequency-related, low-frequency-unrelated and low-frequency-related ambiguous words. Participants completed translation recognition and production tests immediately after learning and again one week later, with flanker and stop-signal tasks interspersed to measure their interference inhibition and response inhibition. The results indicated that inhibitory control, particularly interference inhibition, significantly aided in learning new meanings when direct knowledge transfer from existing knowledge was unfeasible. This research enhances our comprehension of individual differences in word learning, offering valuable perspectives for broader theories of word learning and targeted educational interventions.