The valorization of Crocus sativus focuses mainly on the plant’s stigma because it is one of the most expensive and valuable spices in the world and has great value in the food, cosmetics, and pharmacological industries. Due to this high stigma value, the other parts of the plant are considered as by-products; our study aimed to evaluate the myorelaxant and antispasmodic activities of the byproducts (tepals and leaves) to compare them with the stigma of the plant. To investigate the myorelaxant and antispasmodic activities of the Crocus sativus on isolated rabbit and rat jejunum, we used an in vitro technic with an organ bath and an isotonic transducer. Our results showed that the STG (hydroethanolic extract of stigmas) and LV (hydroethanolic extract of leaves) had a moderate myorelaxant effect with IC50 = 6.61 ± 1.5 and 5.08 ± 0.45 mg/ml, respectively. TPL (hydroethanolic extract of tepals) had a significant ( p ˂ 0.001 ) inhibitory effect on the amplitude of the rabbit jejunum basic contractions with an IC50 = 1.36 ± 0.15 mg/ml. TPL also caused a significant ( p ˂ 0.001 ) antispasmodic activity depending on the dose of the contraction induced by CCh (10−6 M) and KCl (25 mM). The antispasmodic effect of the TPL is slightly altered in the presence of nifedipine by a percentage of 26.8%. This difference is statistically significant ( p ˂ 0.01 ). Therefore, the extract could induce the inhibitory effect on L-type voltage-dependent Ca2+ channels, but not on the guanylate cyclase and nitric oxide pathways. That confirmed that the TPL has a comparable effect to the verapamil. The HPLC-DAD analysis of various parts of C. sativus shows that the three extracts contain the kaempferol flavanol compound, the STG also was revealed to be rich in carotenoids crocin, and these isomers are trans and cis-crocin, safranal, and picrocrocin. In contrast, the TPL revealed the presence of isorhamnetin and quercetin, but the LV was rich in hesperidin and mangiferin. In conclusion, this study supports the traditional use of this plant to treat digestive problems and will allow us to explore future possibilities for treating bowel spasms using natural molecules derived from saffron.