Analyses of anthropogenic and natural gamma-ray emitters in the environment require high sensitive detector systems operating in coincidence-anticoincidence modes. Thanks to an excellent energy resolution and a high efficiency, large volume HPGe detectors have been widely used in low-level gamma-ray spectrometry. In the present paper we discuss the characteristics of single and coincidence (HPGe-NaI(Tl)) arrangements suitable for analysis of environmental samples containing cascade gamma-ray emitters (e.g., 60Co), positron emitters (e.g., 22Na) and single gamma-ray emitters (e.g., 137Cs). The detectors were placed in a large volume shields consisting of iron, lead and copper layers. The reduction of background for the single gamma-ray spectrometer is between 60 and 250, depending on the gamma-ray energy. As an improvement of the apparatus, low detection limits for analysis of 137Cs (0.3 Bq•kg−1) and 60Co (0.1 Bq•kg−1) in environmental samples, respectively, have been obtained.