The design of new remediation strategies and materials for treating saline–alkaline soils is of fundamental and practical importantance for many applications. Conventional soil remediation strategies mainly focus on the development of fertilizers or additives for water, nutrient, and heavy metal managements in soils, but they often overlook a soil sensing function for early detection of salinization/alkalization levels toward optimal and timely soil remediation. Here, new smart soils, structurally consisting of the upper signal soil and the bottom hygroscopic bed and chemically including zwitterionic, thermo‐responsive poly(NIPAM‐co‐VPES) and poly(NIPAM‐co‐SBAA) aerogels in each soil layer are formulated. Upon salinization, the resultant smart soils exhibit multiple superior capacities for reducing the soil salinity and alkalinity through ion exchange, controlling the water cycling, modulating the degradation of pyridine‐base ligands into water‐soluble, nitrogenous salts‐rich ingredients for soil fertility, and real‐time monitoring salinized soils via pH‐induced allochroic color changes. Further studies of plant growth in smart soils with or without salinization treatments confirm a synergy effect of soil remediation and soil sensing on facilitating the growth of plants and increasing the saline–alkaline tolerance of plants. The esign concept of smart soils can be further expanded for soil remediation and assessment.