Various modification methods of halloysite and their applications as modifiers of carbon paste electrodes (CPEs) have been presented. CPEs were modified by the addition of different halloysite materials and were prepared for detection of phenol (Ph) and 4-chlorophenol (4-CP). The electrochemical behavior of these materials was investigated employing cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The modifier was found to enhance the electroactive surface area and the peak current in comparison to the bare carbon paste electrodes. The range of observed changes of these parameters significantly depends on method chosen for halloysite modification.