Monitoring the biochemical pigment contents in individual plants is crucial for assessing their health statuses and physiological states. Fast, low-cost measurements of plants' biochemical traits have become feasible due to advances in multispectral imaging sensors in recent years. This study evaluated the field application of proximal multispectral imaging combined with feature selection and regressive analysis to estimate the biochemical pigment contents of poplar leaves. The combination of 6 spectral bands and 26 vegetation indices (VIs) derived from the multispectral bands was taken as the group of initial variables for regression modeling. Three variable selection algorithms, including the forward selection algorithm with correlation analysis (CORR), recursive feature elimination algorithm (RFE), and sequential forward selection algorithm (SFS), were explored as candidate methods for screening combinations of input variables from the 32 spectral-derived initial variables. Partial least square regression (PLSR) and nonlinear support vector machine regression (SVR) were both applied to estimate total chlorophyll content (Chla+b) and carotenoid content (Car) at the leaf scale. The results show that the nonlinear SVR prediction model based on optimal variable combinations, selected by SFS using multiple scatter correction (MSC) preprocessing data, achieved the best estimation accuracy and stable prediction performance for the leaf pigment content. The Chla+b and Car models developed using the optimal model had R2 and RMSE predictive statistics of 0.849 and 0.825 and 5.116 and 0.869, respectively. This study demonstrates the advantages of using a nonlinear SVR model combined with SFS variable selection to obtain a more reliable estimation model for leaf biochemical pigment content.