The objective of this research was to assess the feasibility of remote sensing (RS) technology, specifically an unmanned aerial system (UAS), to estimate Bambara groundnut canopy state variables including leaf area index (LAI), canopy chlorophyll content (CCC), aboveground biomass (AGB), and fractional vegetation cover (FVC). RS and ground data were acquired during Malaysia’s 2018/2019 Bambara groundnut growing season at six phenological stages; vegetative, flowering, podding, podfilling, maturity, and senescence. Five vegetation indices (VIs) were determined from the RS data, resulting in single-stage VIs and cumulative VIs (∑VIs). Pearson’s correlation was used to investigate the relationship between canopy state variables and single stage VIs and ∑VIs over several stages. Linear parametric and non-linear non-parametric machine learning (ML) regressions including CatBoost Regressor (CBR), Random Forest Regressor (RFR), AdaBoost Regressor (ABR), Huber Regressor (HR), Multiple Linear Regressor (MLR), Theil-Sen Regressor (TSR), Partial Least Squares Regressor (PLSR), and Ridge Regressor (RR) were used to estimate canopy state variables using VIs/∑VIs as input. The best single-stage correlations between canopy state variables and VIs were observed at flowering (r > 0.50). Moreover, ∑VIs acquired from vegetative to senescence stage had the strongest correlation with all measured canopy state variables (r > 0.70). In estimating AGB, MLR achieved the best testing performance (R2 = 0.77, RMSE = 0.30). For CCC, RFR excelled with R2 of 0.85 and RMSE of 2.88. Most models performed well in FVC estimation with testing R2 of 0.98–0.99 and low RMSE. For LAI, MLR stood out in testing with R2 of 0.74, and RMSE of 0.63. Results demonstrate the UAS-based RS technology potential for estimating Bambara groundnut canopy variables.