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In attempting to address problems of water quality, the analyst is keenly aware of the increasing number of parameters for which test methods must be developed. Moreover, the legal pressure of regulation and the economic pressure of process control ensure that the numbers of analyses for each parameter will increase, while maximum allowable limits will decrease. Faced with these restrictions, the water chemist must be prepared to evaluate the advantages and limitations of available techniques, so needed information can be provided in a cost-effective manner. An intelligent match of technique with measurement need may sound obvious but will work to avoid problems only when it is applied. This chapter, it is hoped, will provide an overview of the use of ion-selective electrodes in water and wastewater analysis. Emphasis will be placed on the practical rather than theoretical aspects of such measurements. Electrodes are useful analytical tools, that should be evaluated as carefully as would any other tool.