An attempt of correlating molecular weight (M,) of recycled high-density polyethylene (HDPE) as measured by size-exclusion chromatography (SEC) with diffuse reflectance near and mid-infrared spectroscopy (NIR/MIR) was made by means of multivariate calibration. The spectral data obtained was also used to extract information about the degree of crystallinity of the recycled resin. Differential scanning calorimetry (DSC) was used as the reference method. Partial leastsquares (PLS) calibration was performed on the MIR and NIR spectral data for prediction of Af, Four PC factors described fully the PLS models. The root-meansquare error of prediction (RMSEP) obtained with MIR data was 360, whereas a RMSEP of 470 was achieved when calibration was carried out on the diffuse reflectance NIR data. A PLS calibration for prediction of degree of crystallinity was performed on the NIR data in the 1100-1900-nm region, but the ability of prediction of this model was poor. However a PLS calibration in the region 2000-2500 nm yield better results. Four PC factors explained the most of the variance in the spectra and the RMSEP was 0.4 wt %.