Cellulose nanofibers hold much promise for enhancing the mechanical properties of composites owing to their uniquely high stiffness and strength. One major issue limiting this performance however is the dispersion and mixing of cellulose nanofibers within thermoplastic resins. A combination of Raman imaging and chemical analysis has been used to quantify the distribution and mixing of cellulose nanocrystals (CNCs) in a polyethylene-matrix composite. Large area spectral imaging provides information about the effect of a compatibilizer – namely poly(ethylene oxide) (PEO) and maleated polyethylene (MAPE) - on the distribution of CNCs in the thermoplastic matrix. High-resolution images enable quantification of the degree of mixing between the CNCs and HDPE. Lower resolution images, but with greater spatial spread, allow quantification of the dispersion of the CNCs. It is shown that the CNCs tend to agglomerate, with little increase in dispersion even with the use of the compatibilizer. A shift in the position of characteristic Raman bands indicates the formation of hydrogen bonding between the PEO compatibilizer and the CNCs, which in turn is thought to affect the distribution of aggregates of the reinforcing phase.