Methods and systems are provided for measuring the zeta potential of macroscopic solid surfaces including and not limited to: porous samples, flat substrates, coarse particles, and granular samples. Methods include: subjecting the sample to an injection of a first aqueous solution at an initial pressure with an initial ion concentration; measuring a first electrical conductivity and a first temperature of the first aqueous solution; measuring a first pH and a second pH of the first aqueous solution immediately before and after passing the first aqueous solution through the sample; measuring a first ion concentration and a second ion concentration of the first aqueous solution immediately before and after passing the first aqueous solution through the sample; and processing the measured data to derive a first zeta potential from the first electrical conductivity and the first temperature.