In modern power transmission and distribution systems, power transformers are critical components and their electrical properties together with service lives are determined by the insulation property of oil-paper insulation. To better apply the frequency domain spectroscopy technique to assess transformer insulation condition, a series of experiments were performed under controlled laboratory conditions. First, this article presents the frequency domain dielectric response measurement results of oil-paper insulation samples under different moisture contents and aging states, and then the extracted frequency dielectric characteristic parameters determined from the imaginary part of relative permittivity (ϵr′′) and dielectric dissipation factor (tanδ) curves are used to assess the moisture contents and aging states of oil-paper insulation. Finally, the quantitative relationships among dielectric characteristic parameters, moisture content, and degree of polymerization are also established. Results show that in the frequency range of 10–3–102 Hz, ϵr′′ and tanδ obviously increase as the moisture content of oil-paper insulation rises, while ϵr′′ and tanδ are very sensitive to aging only in 10–3–10–1 Hz. Consequently, ϵr′′ and tanδ in different frequency ranges can be used to distinguish the influences of moisture content and aging state on frequency domain spectroscopy measurement results.