The present investigation describes the effect of the spasmolytic benzylbenzoates 1–9 from Brickellia veronicifolia on CaM using a functional in vitro enzymatic assay. Bovine brain PDE1 was used as a monitoring enzyme. The most active natural inhibitors of the system CaM–PDE1 were benzyl benzoates 3–5, which inhibited the activity of PDE1 in a concentration-dependent manner. In addition, three series of analogs of compound 4, ...