Within the scope of nonlinear optics, optical power limiting (OPL) materials are commonly regarded as an important class of compounds which can protect the delicate optical sensors or human eyes from sudden exposure to damaging intense laser beams. Recent efforts have been devoted to developing organometallic acetylide complexes, dendrimers and polymers as high performance OPL materials of the next generation which can favorably optimize the optical limiting/transparency trade-off issue. These metallated materials offer a new avenue towards a new family of highly transparent homo- and heterometallic optical limiters with good solution processability which outperform those of current state-of-the-art visible-light-absorbing competitors such as fullerenes, metalloporphyrins and metallophthalocyanines. This critical review aims to provide a detailed account on the recent advances of these novel OPL chromophores. Their OPL activity was shown to depend strongly on the electronic characters of the aryleneethynylene ligand and transition metal moieties as well as the conjugation chain length of the compounds. Strategies including copolymerization with other transition metals, change of structural geometry, use of a dendritic platform and variation of the type and content of transition metal ions would strongly govern their photophysical behavior and improve the resulting OPL responses. Special emphasis is placed on the structure–OPL response relationships of these organometallic acetylide materials. The research endeavors for realizing practical OPL devices based on these materials have also been presented. This article concludes with perspectives on the current status of the field, as well as opportunities that lie just beyond its frontier (106 references).