Compared to seeds and mature tissues, sprouts are well known for their higher nutritive and biological values. Fruits of Pimpinella anisum (anise) are extensively consumed as food additives; however, the sprouting-induced changes in their nutritious metabolites are hardly studied. Herein, we investigated the bioactive metabolites, phytochemicals, and antioxidant properties of fruits, sprouts (9-day-old), and mature tissue (5-week-old) of anise under laser irradiation treatment (He-Ne laser, 632 nm). Laser treatment increased biomass accumulation of both anise sprouts and mature plants. Bioactive primary (e.g., proteins and sugars) and secondary metabolites (e.g., phenolic compounds), as well as mineral levels, were significantly enhanced by sprouting and/or laser light treatment. Meanwhile, laser light has improved the levels of essential oils and their related precursors (e.g., phenylalanine), as well as enzyme activities [e.g., O–methyltransferase and 3-Deoxy-D-arabino-heptulosonate-7-phosphate synthase (DAHPS)] in mature tissues. Moreover, laser light induced higher levels of antioxidant and anti-lipidemic activities in sprouts as compared to fruits and mature tissues. Particularly at the sprouting stage, anise was more responsive to laser light treatment than mature plants.