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In this review, the problem of microbiological infestation of buildings was discussed. The techniques of detection were described as well, with special attention drawn to the rapid-early detection methods based on gas sensor arrays. The physical and chemical conditions of the building environment conducive to the development of microorganisms and the technical conditions influencing the problem of microbiological infestation were investigated. Additionally, the harmful effects on human health caused by the microbiological contamination were discussed, with a short review of particular groups of microorganisms causing sick building syndrome. Among the detection techniques, the traditional microbiological techniques as well as the molecular and chemical methods were presented. Different designs of the gas sensor arrays together with the various techniques of analyzing the received multidimensional signal were described, analyzed, and compared in detail.