[Caution! Incautious modification of CPU and memory voltage can easily damage your components.]
If you have reached the upper limit of your PC's stock overclocking potential, consider bumping up the voltage delivered to the processor and/or the memory. By increasing the amount of voltage available to these components, you can increase their overclocked stability. Unfortunately increasing the voltage also increases the heat produced, especially in the case of the processor.
While increasing the voltage slightly generally results in a better overclock, increasing the voltage too much will simply result in a locked-up PC due to overheating, or burnt out circuits. Definitely a case of diminishing returns, unless you invest in a better cooling solution (which is beyond the scope of this article).
Be sure to increase voltage only in single increments. Once you have increased CPU voltage, experiment with overclocking the CPU and FSB again to see if you can push the system farther. It is unlikely that you will see much benefit past one or two voltage increments, especially with a stock heatsink.