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Plant traits are often measured in the field or laboratory to characterize stress responses. However, direct measurements are not always cost effective for broader sampling efforts, whereas indirect approaches such as reflectance spectroscopy could offer efficient and scalable alternatives. Here, we used field spectroscopy to assess whether (1) existing vegetation indices could predict leaf trait responses to heat stress, or if (2) partial least squares regression (PLSR) spectral models could quantify these trait responses. On several warm, sunny days, we measured leaf trait responses indicative of photosynthetic mechanisms, plant water status, and morphology, including electron transport rate (ETR), photochemical quenching (qP), leaf water potential (Ψleaf), and specific leaf area (SLA) in 51 urban trees from nine species. Concurrent measures of hyperspectral leaf reflectance from the same individuals were used to calculate vegetation indices for correlation with trait responses. We found that vegetation indices predicted only SLA robustly (R2 = 0.55), while PLSR predicted all leaf trait responses of interest with modest success (R2 = 0.36 to 0.58). Using spectral band subsets corresponding to commercially available drone-mounted hyperspectral cameras, as well as those selected for use in common multispectral satellite missions, we were able to estimate ETR, qP, and SLA with reasonable accuracy, highlighting the potential for large-scale prediction of these parameters. Overall, reflectance spectroscopy and PLSR can identify wavelengths and wavelength ranges that are important for remote sensing-based modeling of important functional trait responses of trees to heat stress over broad ranges.