Advanced technologies for improved nitrogen (N) fertilizer management are paramount for sustainably meeting future food demands. Green laser systems that measure pulse return intensity can provide more reliable information about foliar N than can traditional passive remote sensing devices during the critical early crop growth stages (e.g., before canopy closure when vegetation and soil signals are spectrally mixed) when further decisions regarding N management can be made. However, current green laser systems are not designed for agricultural applications and only employ a single green laser wavelength, which may limit applications because many factors that require normalization techniques can affect pulse return intensity. Here, we describe the design of a tractor-mountable, green (532nm)- and red (658nm) dual wavelength laser system and evaluate the potential of an additional red reference wavelength to improve laser based estimates of foliar N by calculating laser spectral indices based on ratio combinations of green laser return intensity (GLRI) and red laser return intensity (RLRI). We hypothesized that such laser spectral indices aid in accounting for factors that confound laser based foliar N estimates including variations in leaf angle, measurement distance, soil returns, and mixed edge returns. Leaf level measurements in winter wheat (Triticum aestivum) revealed that the two laser spectral indices improved the relationship with foliar N (r2>0.71, RMSE<0.28%) compared to the sole use of GLRI (r2=0.47, RMSE=0.38%). Laboratory measurements also showed that laser spectral indices reduced the effect of measurement distance on laser readings and allowed leaf returns to be better separated from edge returns and soil returns. However, laboratory measurements showed that laser spectral indices did not account for variations in leaf angle, possibly explaining the weak relationships (r2<0.36, RMSE=0.49%) between foliar N and laser spectral indices observed when employing the laser system under field conditions. In fact, the strongest relationship at the field canopy level was shown for GLRI (r2=0.65, RMSE=0.37%) alone. Laboratory measurements suggest that the better performance of GLRI compared to ratio-based laser spectral indices may result from pronounced differences in the leaf-level bidirectional reflectance distribution factor (BRDFleaf) between the green and red laser wavelengths, thus confounding leaf angle effects so that they are not cancelled when calculating laser spectral indices. This finding suggests that the small spot size of the laser pulses (⩽5mm diameter) interacts with BRDFleaf at very fine scales, therefore causing differential, wavelength-specific scattering effects. Additional study of BRDFleaf at the mm scale is therefore warranted, and should be carefully considered in future development and use of multi-wavelength laser systems for remotely sensing foliar biochemistry.