A series of potassium titanyl phosphate single crystals doped with zinc (KTP: Zn) is grown by spontaneous flux crystallization. Their properties and the way the additive is implanted in the crystal lattice are studied. The inclusion of zinc atoms in the KTP structure is evidenced by the data of chemical analysis and the results of studies of electrophysical properties (the growth of conductivity and increase of relaxation anomalies). Precision X-ray diffraction studies of KTP: Zn single crystals reveal changes in the channel of the structure which correlate with the physical properties of this crystal series. No substitution of zinc atoms for titanium, phosphorus, or potassium atoms is found in the structure. Zinc atoms can be located at structural defects, domain walls, and the crystal surface.