Mercury intrusion capillary pressure (MICP), nuclear magnetic resonance (NMR), routine core analysis, thin sections, and scanning electron microscope (SEM) analysis were used to gain insight into the pore structure of the Eocene Sha-3 (the third member of the Shahejie formation) low-permeability sandstones in the Raoyang sag, including pore type, pore geometry, and pore size. Quantitative NMR parameters and petrophysical properties were integrated to build up the relationship between microscopic pore structure and macroscopic performance. The pore systems of Sha-3 sandstones are dominantly of residual intergranular pores, intragranular dissolution pores, and intercrystallite micropores associated with authigenic clay minerals. The high threshold pressure and low mercury withdrawal efficiencies from MICP analysis indicate the poor pore connectivity and strong heterogeneous. Both uni- and bimodal transverse relaxation time (T-2) spectrum can be found because of the coexistence of small and large pores, and the T-2 of major pore size occurring at about 1.0 to 100 ms. The Sha-3 sandstones have a relatively high irreducible water content and short T-2 components in the T-2 range. Long T-2 components can only be observed in samples rich in large pores or microfractures. T-2gm (the geometric mean of the T-2 distribution) correlates well with irreducible water saturation and permeability. A methodology for pore structure classification is presented integrating NMR parameters of T-2gm, bulk volume of immovable fluid (BVI), and petrophysical parameters such as reservoir quality index (RQI) and permeability. Consequently, four types of pore structures (types A, B, C, and D) are identified, and characteristics of individual pore structure are summarized. The comprehensive analysis of NMR measurements combined with thin sections, SEM and MICP analysis is useful for describing microscopic pore structure, which is important to maintaining and enhancing petroleum recovery in low-permeability sandstone reservoirs.