The research object was three-layer reinforced precast concrete enclosure structures. The structures consist of heavy concrete B25 in the external layers and polystyrene concrete B1 in the internal layer. The stress–strain state of precast concrete structures during crack formation was studied by considering the influence of contact interlayers between different types of concretes. Stereoscopic microscopy and scanning electron microscopy were used in the experimental study of multilayer concrete blocks. Samples were made with a varied break time from 30 min to two hours between the previous and the next concrete layer placings. The experimental results showed that the contact interlayer with mutual penetration of aggregates into the adjacent concrete layers is formed in the successive layer-by-layer placing of various concretes. The thickness of the contact interlayer was up to 1 cm. The contact interlayer affects the solidity of the concrete layers’ connection and the structure’s stress–strain state. A model and method for calculating cracking in three-layer reinforced concrete structures with contact interlayers based on analytical and numerical calculations are proposed. Experimental data confirm the proposed calculation method. The results of three-layer reinforced concrete beams calculations show that: (i) the difference of the moment during crack formation in three-layer reinforced concrete beams schemes with and without taking into account the contact interlayer can reach 9.9%; (ii) the moment during crack formation obtained according to the proposed method is greater than that obtained according to the scheme of the cross-section conversion from 7.4% to 9.1%.