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This study evaluated the effects of two chlorophyll derivatives, sodium copper chlorophyllin (Cu‐Chl) and sodium iron chlorophyllin (Fe‐Chl), on the bond strength between a self‐curing luting agent (4‐META/MMA‐TBB resin) and dentin. Five aqueous primers containing 35% 2‐hydroxyethylmethacrylate with 0.007% Cu‐Chl, 0.07% Cu‐Chl, 0.007% Fe‐Chl, 0.07% Fe‐Chl, or neither Cu‐Chl nor Fe‐Chl (no‐Chl) were prepared. The extracted human dentin surfaces were etched with 10% phosphoric acid (10PA), primed, and bonded to a resin block using the 4‐META/MMA‐TBB resin. A conventional etching agent (10‐3) and 10PA without primer (PA/no‐primer) were used as controls. The microtensile bond strength was determined after 48 h. The arithmetic medians for 20 stick specimens were calculated and statistically analyzed using a nonparametric Steel‐Dwass test (α = 0.05). The maximum bond strength was achieved in the 0.007% Cu‐Chl group, followed by those in the 0.07% Cu‐Chl, 0.07% Fe‐Chl, 10‐3, 0.007% Fe‐Chl, no‐Chl, and PA/no‐primer groups. No significant difference was observed between 0.007% Fe‐Chl, 0.07% Fe‐Chl, and 10‐3. The bond strength to dentin etched with 10PA was influenced by the type and concentration of the chlorophyll derivatives applied. Cu‐Chl rather than Fe‐Chl should be useful as a component of surface treatment agents for bonding 4‐META/MMA‐TBB resin to dentin. [ABSTRACT FROM AUTHOR]