With two independent pore systems (intralayer sinusoidal channels and interlayer supercages) and external 12 membered-ring (MR) cups, H-MCM-49 was selected as the acidic support for upgrading palmitic acid to jet-fuel-range hydrocarbons via simultaneous hydro-deoxygenation, hydrocracking, and hydroisomerization. Compared to other zeolites, H-MCM-49 showed better selectivity toward cracking and isomerizing products (C-12 -C(14 )alkanes). Postsynthesis of H-MCM-49 could tailor acidity and catalytic performance to produce more C-12-C-14 cracking and isoalkane products. Ni/H-MCM-49 bifunctional catalysts restrained the acidcatalyzed reactions to some extent because of enhancement in hydro-deoxygenation over Ni particles, leading to the decrease in appropriate cracking of C-12-C-14 alkanes' and isoalkanes' selectivity. Ni/H-MCM-49 bifunctional catalysts exhibited excellent catalytic stability on activity and selectivity of target products, which opened a novel tailoring pathway over zeolites with independent pore systems.