The formation of wormlike micelles in aqueous solutions of an amino acid‐based surfactant, sodium lauroyl sarcosinate (LS) and a zwitterionic surfactant, cocamidopropyl betaine (CAPB) has been investigated. Holding the total concentration of LS and CAPB constant at 12 wt%, the synergistic effects of mass ratio of CAPB and LS and pH of the micelle solution on rheological behaviors of CAPB/LS micelles were studied. The viscosity of CAPB/LS micelle systems with a mass ratio from 4:8 to 9:3 increases to maximum values and then decreases as pH increases from 4.0 to 5.6. The maximum viscosity of the transparent CAPB/LS micelle solution is nearly 5500 mPa·s with a mass ratio of CAPB/LS = 8:4 at pH 5.10. It is suggested that the proper pH for CAPB and LS to form wormlike micelles should be close to the isoelectric point of the CAPB/LS solution. The results of thixotropy measurements show that the appropriate mass ratio of CAPB/LS can improve the stability of the network structure of wormlike micelles. In addition, viscosity curves of CAPB/LS wormlike micelles follow a nonlinear co‐rotational Jeffreys model, and the linear viscoelasticity of CAPB/LS wormlike micelles can be described by a linear viscoelastic Jeffreys model. The network of wormlike micelles is confirmed by Cryo‐TEM images.
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