Antireflection coatings (ARC) are essential for various optical components including such made of plastics for high volume applications. However, precision coatings on plastics are rather challenging due to typically low adhesion of the coating to the substrate. In this work, optimization of the atomic layer deposition (ALD) processes towards conformal optical thin films of Al2O3, TiO2 and SiO2 on poly(methyl methacrylate) (PMMA) has been carried out and a five-layer ARC is demonstrated. While the uncoated PMMA substrates have a reflectance of nearly 8% in the visible (VIS) spectral range, this is reduced below 1.2% for the spectral range of 420–670 nm by applying a double-side ARC. The total average reflectance is 0.7%. The optimized ALD coatings show a good adhesion to the PMMA substrates even after the climate test. Microscopic analysis on the cross-hatch areas on PMMA after the climate test indicates very good environmental stability of the ALD coatings. These results enable a possible route by ALD to deposit uniform, crack free, adhesive and environmentally durable thin film layers on sensitive thermoplastics like PMMA.