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Four novel indane derivatives, anisotindans A–D (<b>1</b>–<b>4</b>), were isolated from the roots of <i>Anisodus tanguticus</i>. Their structures were established using comprehensive spectroscopic analyses, and their absolute configurations were determined by electronic circular dichroism (ECD) calculations and single-crystal X-ray diffraction analyses. Anisotindans C and D (<b>3</b> and <b>4</b>) are two unusual indenofuran analogs. ABTS^•+ and DPPH^•+ assays of radical scavenging activity reveal that all compounds (<b>1</b>–<b>4</b>) are active. Specifically, the ABTS^•+ assay results show that anisotindan A (<b>1</b>) exhibits the best antioxidant activity with an IC₅₀ value of 15.62 ± 1.85 μM (vitamin C, IC₅₀ = 22.54 ± 5.18 μM).