This study provides validity evidence for the Capture-Recapture (CR) method, borrowed from ecology, as a measure of second language (L2) productive vocabulary size (PVS). Two separate “captures” of productive vocabulary were taken using written word association tasks (WAT). At Time 1, 47 bilinguals provided at least 4 associates to each of 30 high-frequency stimulus words in English, their first language (L1), and in French, their L2. A few days later (Time 2), this procedure was repeated with a different set of stimulus words in each language. Since the WAT was used, both Lex30 and CR PVS scores were calculated in each language. Participants also completed an animacy judgment task assessing the speed and efficiency of lexical access. Results indicated that, in both languages, CR and Lex30 scores were significantly positively correlated (evidence of convergent validity). CR scores were also significantly larger in the L1, and correlated significantly with the speed of lexical access in the L2 (evidence of construct validity). These results point to the validity of the technique for estimating relative L2 PVS. However, CR scores are not a direct indication of absolute vocabulary size. A discussion of the method’s underlying assumptions and their implications for interpretation are provided.