The advancement of mobile technologies enables students to learn English without being limited by space and time. Recent studies investigated affective factors and personality traits in English as a Foreign Language (EFL) learning. However, few studies have explored the mediating factors on the relationship between their perfectionism and English learning burnout levels in mobile learning contexts. To fill the gap, this study investigated the association between self-oriented perfectionism and English learning burnout under the influence of grit and language learning anxiety among Chinese college-level EFL learners (N = 544) through the means of structural equation modeling. The results indicated that 1) self-oriented perfectionism did not directly predict English learning burnout in mobile learning contexts, but the relationship was mediated by grit and language learning anxiety; 2) self-oriented perfectionism positively predicted grit, whereas grit negatively predicted English learning anxiety; 3) grit negatively predicted reduced academic efficacy in mobile EFL learning.