For double negative materials (DNMs), these are usually observed in artificial metamaterials or some metal/ceramic composites. Here, an interesting negative permittivity behavior of single-phase perovskite La1−xSrxMnO3 (LSMO) is found. The LSMO bulks with an x value of 0.2 or 0.5 were prepared by a sol–gel/sintering process. From microstructure characterization, the bulks are nearly in single phase and the major phase belongs to the perovskite structure; meanwhile, the bulks are of high density. Furthermore, the experimental data of the plasma-like negative permittivity are fitted well by a lossy Drude model, suggesting a plasma frequency of 3.85 GHz (x = 0.5). The complex permeability of LSMO presents a negative susceptibility (μ′ < 1) at a frequency range of 0.2–1 GHz (x = 0.2) and 0.6–1 GHz (x = 0.5). These results have important implications for the realization of double negative properties in single-phase LSMO as a promising candidate for DNMs.