In general, a high voltage (HV) substation can be made up of multiple insulation subsystems: an air insulation subsystem (AIS), gas insulation subsystem (GIS), liquid insulation subsystem (power transformers), and solid insulation subsystem (power cables), all of them with their grounding structures interconnected and linked to the substation earth. Partial discharge (PD) pulses, which are generated in a HV apparatus belonging to a subsystem, travel through the grounding structures of the others. PD analyzers using high-frequency current transformer (HFCT) sensors, which are installed at the connections between the grounding structures, are sensitive to these traveling pulses. In a substation made up of an AIS, several non-critical PD sources can be detected, such as possible corona, air surface, or floating discharges. To perform the correct diagnosis, non-critical PD sources must be separated from critical PD sources related to insulation defects, such as a cavity in a solid dielectric material, mobile particles in SF6, or surface discharges in oil. Powerful diagnostic tools using PD clustering and phase-resolved PD (PRPD) pattern recognition have been developed to check the insulation condition of HV substations. However, a common issue is how to determine the subsystem in which a critical PD source is located when there are several PD sources, and a critical one is near the boundary between two HV subsystems, e.g., a cavity defect located between a cable end and a GIS. The traveling direction of the detected PD is valuable information to determine the subsystem in which the insulation defect is located. However, incorrect diagnostics are usually due to the constraints of PD measuring systems and inadequate PD diagnostic procedures. This paper presents a diagnostic procedure using an appropriate PD analyzer with multiple HFCT sensors to carry out efficient insulation condition diagnoses. This PD procedure has been developed on the basis of laboratory tests, transient signal modeling, and validation tests. The validation tests were carried out in a special test bench developed for the characterization of PD analyzers. To demonstrate the effectiveness of the procedure, a real case is also presented, where satisfactory results are shown.