Chickpea protein isolate (CPI) emulsion gels suffered from poor elasticity and loose structure, which greatly limited their application and development. This work aimed to investigate the effect of cellulose nanofibrils (CNFs) on the intermolecular interactions, protein structure, gel properties, and microstructure of CPI emulsion gels. Results showed that CNFs enhanced the hydrophobic interactions, electrostatic interactions, and hydrogen bonding of the CPI emulsion gels, and contributed to the transition of the secondary structure of CPI from α-helix to β-sheet structure. CPI-CNFs emulsion gels exhibit better textural properties, rheological properties and water holding capacity compared to CPI emulsion gels. Gel strength increased from 40.67 g to 56.26 g and hardness increased from 42.95 g to 60.67 g. Furthermore, scanning electron microscopy showed that the CPI emulsion gel structures were transformed from rough and porous to uniform and dense with the addition of CNFs. This study indicated that CNFs will help improve the properties of CPI emulsion gels with wide applications in the food field.