<jats:title>Abstract</jats:title><jats:p>Ten new phenolic compounds including the six neolignans <jats:bold>1</jats:bold>–<jats:bold>3</jats:bold> and <jats:bold>6</jats:bold>–<jats:bold>8</jats:bold> and four caffeoyl derivatives, <jats:italic>i.e., myo</jats:italic>‐inositol 1‐caffeate (<jats:bold>9</jats:bold>), <jats:italic>myo</jats:italic>‐inositol 6‐caffeate (<jats:bold>10</jats:bold>), <jats:italic>myo</jats:italic>‐inositol 5‐caffeate (<jats:bold>11</jats:bold>), and paucine 3′‐<jats:italic>β</jats:italic>‐<jats:sc>D</jats:sc>‐glucopyranoside (<jats:bold>12</jats:bold>) were isolated from the whole plants of <jats:italic>Selaginella moellendorffii</jats:italic> (caffeic acid=3‐(3,4‐dihydroxyphenyl)prop‐2‐enoic acid). Their structures were established by spectroscopic and chemical methods.