While previous research emphasized the effects of self-regulated learning on academic achievement, this study expands the scope of self-regulated learning to career-development processes. This study examines how young people build their employability through self-regulated learning processes and whether career maturity might be a critical antecedent of self-regulated learning processes. Results from 257 undergraduates in Taiwan indicate that both metacognitive and motivational self-regulated learning contribute to young people's perceived employability. Early career maturity is associated with metacognitive and behavioral self-regulated learning. Most importantly, metacognitive self-regulated learning serves as a mediator in the relationship between career maturity and perceived employability.