Cellulose nanocrystals (CNCs) are composed of chiral cellulose units, which form chiral nematic liquid crystals in water that, upon drying, self-assemble to more complex spiral chiral sheets. This secondary structure arrangement is found to change with an external magnetic or electric field. Here, we show that one of the basic organization driving forces is electron spin, which is produced as the charge redistributes in the organization process of the chiral building blocks. It is important to stress that the electron spin-exchange interactions supply the original driving force and not the magnetic field per se. The results present the first utilization of the chiral-induced spin selectivity (CISS) effect in sugars, enabling one to regulate the CNC bottom-up fabrication process. Control is demonstrated on the organization order of the CNC by utilizing different magnetization directions of the ferromagnetic surface. The produced spin is probed using a simple Hall device. The measured Hall resistance shows that the CNC sheets' arrangement is affected during the first four hours as long as the CNC is in its wet phase. On introducing the 1,2,3,4-butanetetracarboxylic acid cross-linker into the CNC sheet, the packing density of the CNC helical structure is enhanced, presenting an increase in the Hall resistance and the chiral state.