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Introduction: University athletes experienced considerable psychological pressure due to the simultaneous demands of competitive sport and academic responsibilities, while systematic psychological preparation remained limited within collegiate sport programs. Objectives: The study aimed to examine the multidimensional structure of competitive pressure, evaluate the effectiveness of a periodized psychological preparation intervention, and validate a composite psychological load monitoring index among university athletes. Methods: A longitudinal quasi-experimental design was employed across two competitive seasons. The sample comprised 312 university athletes from twenty-eight sports disciplines. Repeated psychological, physiological, and performance-related measures were collected before, during, and after a sixteen-week multimodal psychological preparation program. Data were analyzed using confirmatory factor analysis and multilevel modeling to assess structural validity, intervention effects, and moderating individual factors. Results: Confirmatory factor analysis supported a three-factor model of competitive pressure, demonstrating excellent fit (comparative fit index = 0.971; Tucker–Lewis index = 0.965; root mean square error of approximation = 0.048). The intervention produced significant improvements in autonomic regulation (β = 0.41), reductions in cognitive anxiety (β = −2.84), and enhanced competitive performance (β = 0.52). Physiological stress reactivity and recovery showed large effect size improvements (d = 1.02–1.53). Maladaptive perfectionism significantly moderated intervention responsiveness. The Psychological Load Index demonstrated high predictive accuracy for performance outcomes (area under the curve = 0.87). Conclusions: The findings demonstrated that structured psychological preparation significantly improved psychological regulation, physiological stress control, and athletic performance. Multimodal monitoring provided superior predictive value compared to single-method assessment, supporting its integration into university sport systems.