The present work describes the preparation of host-guest complex formation-responsive liquid marbles (LMs) composed of a water droplet and hydrophobic adamantane (AD) powder. The importance of hydrophobic and hydrophilic balance to the stability of LM was demonstrated with this system. The hydrophobic AD powder formed an amphiphilic system upon formation of a host-guest complex with methyl-beta-cyclodextrin (CD). Although the LM was stable for more than one hour on the water surface, it collapsed on the surface of a CD aqueous solution within a few minutes due to formation of the AD-CD complex.