The influence of polymer composition on the sensitivity towards nitrite (NO2−) and nitric oxide (NO) of a series of 19 polymeric hydrogel films has been studied. The polymers, based on the hydrophilic monomer 2-hydroxyethylmethacrylate (HEMA), are able to encapsulate the colorimetric indicator 1,2-diaminoanthraquinone (DAQ) and to respond to NO2− and NO by visual changes. In the case of nitrite, the calculated limits of detection (LOD) for two of the polymeric sensors (10 μM) are very close to the sensitivity estimated for free DAQ in solution (LOD 5 μM), but with the advantage of a solid supported sensor with the format of a disposable test-strip made with affordable starting chemicals. The results are interpreted taking into account the nature and proportions of monomers and cross-linkers used for the synthesis of polymers. Key factors for obtaining sensitive materials are the hydrophilic character of the film along with the utilization of low levels of cross-linker and the use of an acidic monomer, like acrylic acid, as a building block.