This paper designs and analyzes the bit-interleaved coded modulation with iterative demapping and decoding (BICM-ID) framework under color-shift-keying (CSK) modulation to achieve spectrally efficient transmissions in visible light communication (VLC) systems. Specifically, we investigate the protograph low-density parity-check (LDPC) codes, bit-to-symbol mapping schemes, and constellation labeling rules in higher-order CSK-aided VLC systems. To fully explore the BICM-ID benefit, we propose an irregular CSK mapping, in which an <inline-formula><tex-math notation="LaTeX">$M$</tex-math></inline-formula>-ary standardized constellation (called <italic>“Standard constellation”</italic>) and a new <inline-formula><tex-math notation="LaTeX">$M$</tex-math></inline-formula>-ary constellation (called <italic>“Target constellation”</italic>) are separately applied to modulate two different coded sub-blocks in a codeword to optimize the error performance of the CSK-aided VLC systems. Furthermore, using a modified protograph extrinsic information transfer (PEXIT) algorithm, we construct two types of protograph LDPC codes (i.e., unpunctured and punctured protograph LDPC codes) that outperform the conventional protograph LDPC codes. Both analytical and simulation results show that the proposed irregular-CSK-mapped BICM-ID employing the new protograph LDPC codes and Target constellation is capable of achieving outstanding performance, and is a promising transmission solution for high-speed VLC applications.