This study explores the relationship between the perceived physical literacy (PL) and physical activity (PA) levels of Hong Kong adolescents by using a cross-sectional study design. A total of 1,945 adolescents aged between 12 and 18, (1,028 male and 917 female) with a mean age of 14.98 (±1.65 years), took part in this study. A Perceived Physical Literacy Instrument (PPLI) and an International Physical Activity Questionnaire for Adolescents (IPAQ-A) were distributed to the participants within the first 15 minutes of PE lessons at their schools. The correlation between perceived PL and PA levels was low but significant (r = 0.227, p < 0.01), as was the correlation between the attributes of PL and PA intensity and the domains of PA (r = 0.067–0.292, p < 0.01). A significant linear equation was computed (F (3, 1941) = 35.679, p < 0.01), with an R2 of 0.052. The metabolic equivalent (MET) minutes representing participants’ predicted PA levels were –5490 + 366.1 (sense of self and self-confidence) + 221.866 (self-expression and communication with others) + 287.748 (knowledge and understanding). Looking at individual factors, the correlation between perceived PL and PA levels showed no significant difference across gender (r male = 0.234; r female = 0.198) but showed a significant difference across grade level (r junior = 0.302; r senior = 0.197), school bands (r band 1 = 0.31; r band 2 = 0.263; r band 3 = 0.191) and socio-economic status (SES) (rlow = 0.225; rmedium = 0.35; rhigh = 0.191). The relationship between perceived PL and PA levels was significantly low but was closely related to the recreational PA, including individual factors such as gender, grade levels, school band and SES. Future studies could focus on school-based PA intervention programmes for perceived PL and the relationship between perceived PL and objective PA levels.