Cellulose nanocrystals (CNCs) derived from native cellulose can self-assemble into liquid crystals (LCs) and preserve the LC alignment in solid films that are attractive for the preparation of optical materials and devices from bottom-up manufacturing. Birefringent aligned CNC films provide the desired phase retardation for a narrow band of wavelengths due to the intrinsic wavelength-dependent birefringence of CNCs. Here, we produce a 1/4 λ achromatic CNC-based waveplate consisting of three layers of birefringent CNC films with phase retardations and slow axis directions, which are calculated by Jones Matrix, with optimized achromatic properties. Three uniform CNC films are prepared by aligning nematic CNC LCs doped with polyethylene glycol on patterned polydimethylsiloxane substrates. The fabricated achromatic waveplate is characterized by measuring the transmission spectra, and its maximum deviation of phase retardation is around 0.06 for the wavelength range of 460–660 nm. The achromatic performance is improved by one order of magnitude compared with the single birefringent CNC films. Our CNC-based achromatic waveplate has good optical homogeneity, flexibility and can be tailored into arbitrary shape.