We present JHK_s photometry, far red spectra, and spectral classifications for an additional 67 L dwarfs discovered by the Two Micron All Sky Survey. One of the goals of this new search was to locate more examples of the latest L dwarfs. Of the 67 new discoveries, 17 have types of L6 or later. Analysis of these new discoveries shows that Hα emission has yet to be convincingly detected in any L dwarf later than type L4.5, indicating a decline or absence of chromospheric activity in the latest L dwarfs. Further analysis shows that 16 (and possibly four more) of the new L dwarfs are lithium brown dwarfs and that the average line strength for those L dwarfs showing lithium increases until type ~L6.5 V, then declines for later types. This disappearance may be the first sign of depletion of atomic lithium as it begins to form into lithium-bearing molecules. Another goal of the search was to locate nearer, brighter L dwarfs of all subtypes. Using absolute magnitudes for 17 L dwarf systems with trigonometric parallax measurements, we develop spectrophotometric relations to estimate distances to the other L dwarfs. Of the 67 new discoveries, 21 have photometric distances placing them within 25 pc of the Sun. A table of all known L and T dwarfs believed to lie within 25 pc—53 in total — is also presented. Using the distance measurement of the coolest L dwarf known, we calculate that the gap in temperature between L8 and the warmest known T dwarfs is less than 350 K and probably much less. If the transition region between the two classes spans a very small temperature interval, this would explain why no transition objects have yet been uncovered. This evidence, combined with model fits to low-resolution spectra of late M and early L dwarfs, indicates that L-class objects span the range 1300 K T_eff 2000 K. The near-infrared color-color diagram shows that L dwarfs fall along a natural, redder extension of the well-known M dwarf track. These near-infrared colors get progressively redder for later spectral types, with the L dwarf sequence abruptly ending near (J-H, H-K_s, J-K_s) ≈ (1.3, 0.8, 2.1).