Pesticides pose a significant threat to nontargeted organisms, and their pervasive use makes avoidance challenging. We employed nitrogen-doped carbon cryogels for the removal of organophosphate pesticides. The materials were synthesized and characterized using SEM, Raman spectroscopy, XPS, and BET analysis. Results revealed mesoporous cryogels with pore diameters ranging from 3 to 13 nm. Interestingly, the specific surface area did not change systematically with increasing nitrogen content. All investigated materials have similar composition and structural disorder. Dimethoate, malathion, and chlorpyrifos removal was investigated under stationary and dynamic conditions. Stationary conditions demonstrated successful removal of aliphatic dimethoate and malathion by all investigated materials. Conversely, the materials with the lowest and highest nitrogen content proved ineffective with aromatic chlorpyrifos. Under dynamic conditions, all materials effectively removed malathion and chlorpyrifos while exhibiting suboptimal performance for dimethoate adsorption. Application of nitrogen-doped carbon cryogels to tap water spiked with pesticides yielded successful results under the same conditions. Toxicity testing of treated samples revealed a consistent decrease in toxicity, indicating that contact with cryogels reduces the initial solution’s toxicity. This result also confirms that material–pesticide interaction does not lead to the formation of more toxic byproducts. The demonstrated efficacy suggests the potential application of these materials in water treatment.