A method for chroma Intra prediction allowing different chroma blocks in a coding unit to use separate chroma Intra prediction modes is disclosed. The method selects chroma Intra prediction modes for a first chroma block and one or more non-first chroma blocks in a current color block, where the first chroma block and at least one non-first chroma block use separate chroma Intra prediction modes. The method may comprise determining candidate mode sets for the first chroma block and the non-first chroma blocks. The method may also comprise signaling information of the chroma Intra prediction modes selected for the first chroma block and said one or more non-first chroma blocks. Furthermore, a method of chroma Intra prediction using one or more cross-chroma linear model Intra prediction modes is disclosed for improving coding efficiency of chroma Intra prediction.