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The surface tensions of xPbO-(100 − x) B2O3 (x = 30–80 mol%) and xBi2O3-(100 − x) B2O3 (x = 0–100 mol%) melts were measured using the ring method over the temperature range 973 to 1373 K. The compositional and temperature dependences of surface tension were investigated. Addition of PbO and Bi2O3 to B2O3 increased the surface tensions of their respective PbO-B2O3 and Bi2O3-B2O3 melts. The surface tension showed a maximum at 60 mol% PbO in the PbO-B2O3 melts and at 70–80 mol% Bi2O3 in the Bi2O3-B2O3 melts. The temperature coefficient of surface tension was examined on the basis of its relationship to the structure, and it was suggested that the temperature coefficient of surface tension decreases with an increasing content of four-coordinated boron.