This paper proposes a setup for a best multisine design method that uses a time-domain optimization. The method is based on minimization of the time-domain error, so its resulting multisine has a very accurate ACLR estimation. This is because its probability distribution and sample-to-sample correlation are close to those of the original signal, which are crucial for the testing of nonlinear power amplifiers. In addition, a hyperbolic-tangent function is introduced to control the ripple of tone magnitudes within signal bandwidth. For the verification, multisines were generated and compared for many aspects such as normalized error, in-band ripple, and ACLR estimation. Test results with different numbers of tones provide supporting evidence that the suggested multisine design has better ripple suppression, by up to 7 dB, and better accuracy, by up to 0.2 dB, when compared to the conventional method. The accuracy of the ACLR was improved by about 5 dB when the number of tones was 4. The suggested method improves the ACLR estimation performance of multisine testing due to its closer resemblance to the target modulation signal.