Promoting students' self-regulatory capacity in vocabulary learning has been one of the instructional goals in language education. Learning strategies and motivational beliefs (e.g., self-efficacy) are the key, interrelated factors of self-regulated learning, which are crucial for learners' academic performance. This study investigated Chinese English Foreign language (EFL) learners' needs in terms of cognitive and metacognitive strategy use, as well as their perceptions and knowledge in vocabulary learning. Both qualitative and quantitative research techniques were applied to collect data with 38 preuniversity Chinese EFL learners studying at University of Malaya. The findings revealed that the students possessed insufficient knowledge of high-frequency words and were deficient in using cognitive deep processing strategies (e.g., semantic grouping, word structure) and metacognitive control strategies (e.g., goal-setting). It also indicated that learners' low self-efficacy and motivation might be due to the lack of strategy knowledge, which in turn affects their strategy performance. The study suggests that there is a pressing need to enhance learners' self-regulation in learning vocabulary through explicit strategy instruction, which emphasizes cognitive, metacognitive, and motivational aspects of learning.