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The factors determining litter decomposition incorporated into C and nutrient cycles were examined as part of a broader study investigating the biogeochemical cycle in forest ecosystems. Litter was collected from five altitudes of Qinghai spruce (Picea crassifolia) woodland stands in the Qilian Mountains and placed in litterbags. These litterbags were installed at the crown center (CC) and crown edge (CE) at different altitudes in Qinghai spruce forests during the growing season to study the effect of litter substrate quality on litter decomposition. Results indicate that at varying altitudes in the growing season, the initial mass loss rate and initial decomposition rate of Qinghai spruce litter showed a nonlinear relationship with altitude. The Olson exponential regression equation showed that the decomposition coefficient (k) was the largest at 3050 m (k = 0.709), and the decomposition coefficient (k) was the smallest at 3250 m (k = 0.476). Meanwhile, the initial decomposition rate was highly correlated with initial litter Ca and Mn concentrations. At the CC and CE at different altitudes in the growing season, the initial mass loss rate of CE was significantly higher than that of CC (p < 0.01), and the initial decomposition rate of CE was markedly faster than that of CC (p < 0.01). The Olson exponential regression equation showed that CE’s decomposition coefficients (k) were larger than those of CC. The initial decomposition rate of CE was highly correlated with initial litter C and Mn concentrations. However, the initial decomposition rate at CC was independent of the litter substrate quality. Finally, we realize that litter decomposition in the early stages is not ultimately determined by a single common factor, but rather the result of multiple factors working together in different orders and strengths. The results lay a foundation for understanding the process and mechanism of litter decomposition in the alpine mountain forest ecosystem and further understanding the structure and function of the ecosystem.