Harvested broccoli is prone to decline in quality with regard to its appearance and nutrition. In this study, freshly harvested broccoli was treated with methyl jasmonate (MeJA) and melatonin (MT) and stored at 20 °C and the changes in sensory qualities and bioactive compounds were analyzed. The control samples began yellowing on day 2, whereas MeJA and MT treatments delayed the yellowing by 2 and 4 days, respectively. Upon yellowing, sweetness and bitterness of control samples increased sharply, accompanied by the accumulation of bioactive compounds, except for sulforaphane; however, no significant change in volatile components was detected. When the samples started losing their green color, MeJA alleviated the bitterness while increasing the sweetness and sulforaphane content. The bitterness, astringency, umami level, and the content of sulfurous volatiles improved significantly in the MT-treated samples. Moreover, these samples showed high antioxidant activity; the protective effect on V_C and carotenoids was extremely significant.