Background: It is known that the consumption of single phytochemicals improves respiratory function in chronic obstructive pulmonary disease (COPD) patients. Since phytochemicals have a synergistic effect on health, a more comprehensive analysis is needed. The aim of this study was to estimate the intake of phytochemicals using the dietary phytochemical index (DPI) and assess their association with respiratory function, inspiratory muscle strength and function, and peripheral muscle strength. Methods: This study was conducted at the Special Hospital for Pulmonary Diseases in Zagreb (September 2023 to May 2024). The DPI was assessed using three 24 h recalls from 71 COPD patients (66.5 ± 8.4 years; 53.5% men). Anthropometric measurements, respiratory function, inspiratory muscle function and strength, and peripheral muscle strength were assessed during pulmonary rehabilitation following standard protocols. Results: Patients were divided into DPI tertiles with mean values of 7.3 ± 3.0, 16.0 ± 3.0, and 32.2 ± 8.8, respectively. After controlling for confounding factors, a significant association was found between DPI tertiles and FEV1 (p-trend < 0.001), FVC (p-trend = 0.002), FEV1/FVC (p-trend < 0.001), MIP (p-trend = 0.012), and MSUE (p-trend = 0.002). In addition, an inverse association was found between DPI tertiles and diaphragm thickness during inhalation (p-trend = 0.012) and exhalation (p-trend = 0.013). Conclusions: This study suggests that a higher intake of phytochemicals could be beneficial in dietary interventions for COPD therapy. Future prospective studies are needed to confirm these findings.