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In the present study, phytochemical investigation, antioxidant potential and quantum study on the dichloromethane (DCM) and ethanol extracts of Araucaria columnaris (G. Forst.) Hook. branches have been carried out. The ethanol extract has higher total bioactive contents as compare with DCM extract such as total polyphenolic contents, total flavonoids contents and total tannin contents. The phytochemical quantification and volatile composition of most bioactive extract (ethanol) has been carried out by RP-HPLC-DAD (9-compounds) and GC-MS (19-compounds). The antioxidant potential was demonstrated using free radical scavenging, phosphomolybdenum, metal chelating and reducing power assays. The ethanol extract has higher antioxidant potential. The Density Functional Theory (DFT) has been carried out on major phytochemicals of ethanol extract. The current findings revealed an excellent concentration of bioactive compounds in A. columnaris (G. Forst.) Hook. branch, which reaffirms the great significance of the current work and benefaction to natural products chemistry.