A critical approach for efficiently deploying Mixture-of-Experts (MoE) models with massive parameters is quantization. However, state-of-the-art MoE models suffer from non-negligible accuracy loss with extreme quantization, such as under 4 bits. To address this, we introduce MiLo, a novel method that augments highly quantized MoEs with a mixture of low-rank compensators. These compensators consume only a small amount of additional memory but significantly recover accuracy loss from extreme quantization. MiLo also identifies that MoE models exhibit distinctive characteristics across weights due to their hybrid dense-sparse architectures, and employs adaptive rank selection policies along with iterative optimizations to close the accuracy gap. MiLo does not rely on calibration data, allowing it to generalize to different MoE models and datasets without overfitting to a calibration set. To avoid the hardware inefficiencies of extreme quantization, such as 3-bit, MiLo develops Tensor Core-friendly 3-bit kernels, enabling measured latency speedups on 3-bit quantized MoE models. Our evaluation shows that MiLo outperforms existing methods on SoTA MoE models across various tasks.