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Four previously undescribed terpenoid glucosides, including one sesquiterpenoid di-glucoside (<b>1</b>), two new iridoid glucosides (<b>2</b>, <b>3</b>), and a new triterpenoid tri-glucoside (<b>4</b>), were isolated from a 70% ethanol extract of the root of <i>Gentiana macrophylla</i> (Gentianaceae), along with eight known terpenoids. Their structures were determined by spectroscopic techniques, including 1D, 2D NMR, and HRMS (ESI), as well as chemical methods. The absolute configuration of compound <b>1</b> was determined by quantum chemical calculation of its theoretical electronic circular dichroism (ECD) spectrum. The sugar moieties of all the new compounds were confirmed to be D-glucose by GC analysis after acid hydrolysis and acetylation. Anti-pulmonary inflammation activity of the iridoids were evaluated on a TNF-α induced inflammation model in A549 cells. Compound <b>2</b> could significantly alleviate the release of proinflammatory cytokines IL-1β and IL-8 and increase the expression of anti-inflammatory cytokine IL-10.