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<i>Campanula takesimana</i> Nakai (Campanulaceae; Korean bellflower) is one of the endemic herbs of Korea. The plant has been used as traditional medicines for treating asthma, tonsillitis, and sore throat in Korea. A hot water extract of the leaves of <i>C. takesimana</i> exhibited a significant inhibitory effect on lipopolysaccharide (LPS)-stimulated prostaglandin E₂ (PGE₂) production. Repetitive chromatographic separation of the hot water extract led to the isolation of three new neolignan glucosides, campanulalignans A–C (<b>1</b>–<b>3</b>), with 15 known compounds (<b>4</b>–<b>18</b>). The structures of new compounds <b>1</b>–<b>3</b> were elucidated by analyzing nuclear magnetic resonance (NMR) spectroscopic data, along with high resolution quadrupole time of flight mass (HR-Q-TOF-MS) spectrometric data. Among the isolates, simplidin (<b>7</b>), 5-hydroxyconiferaldehyde (<b>11</b>), icariside F₂ (<b>12</b>), benzyl-<i>α</i>-<span style="font-variant: small-caps;">l</span>-arabinopyranosyl-(1″→6′)-<i>β</i>-<span style="font-variant: small-caps;">d</span>-glucopyranoside (<b>13</b>), and kaempferol 3-<i>O</i>-<i>β</i>-<span style="font-variant: small-caps;">d</span>-apiosyl (1→2)-<i>β</i>-<span style="font-variant: small-caps;">d</span>-glucopyranoside (<b>15</b>) were isolated from the Campanulaceae family for the first time. The isolates (<b>1</b>, <b>2</b>, and <b>4</b>–<b>18</b>) were assessed for their anti-inflammatory effects on LPS-stimulated PGE₂ production on RAW 264.7 cells. 7<i>R</i>,8<i>S</i>-Dihydrodehydrodiconiferyl alcohol (<b>5</b>), 3′,4-<i>O</i>-dimethylcedrusin 9-<i>O</i>-<i>β</i>-glucopyranoside (<b>6</b>), pinoresinol di-<i>O</i>-<i>β</i>-<span style="font-variant: small-caps;">d</span>-glucoside (<b>8</b>), ferulic acid (<b>10</b>), 5-hydroxyconiferaldehyde (<b>11</b>), and quercetin (<b>18</b>) showed significant inhibitory effects on LPS-stimulated PGE₂ production.